Practical synthetic approaches to several new "purine-like" C-nucleosides are described. These substances are structurally related to several new purine nucleoside antimetabolites synthesized recently in our laboratory, namely the 9-deazapurine C-nucleosides and their thieno analogs which have exhibited exceptional growth inhibitory activities. Rationales are offered which are based on: a) the demonstrated anticancer activities of the lead C-nucleosides, and b) other biochemical considerations. It is suggested that several of the candidates may possess higher chemotherapeutic indices than the original lead compounds and that some may exhibit useful antiviral properties. "In-house" biochemical and biological studies for the proper antitumor evaluation of all target C-nucleosides are described. Relationships between chemical structures and anticancer activity should be ascertainable from these investigations.